The effect of gas additives on reactive species and bacterial inactivation by a helium plasma jet

In this paper,the influences of gas doping(O_2,N_2,Air)on the concentrations of reactive species and bactericidal effects induced by a He plasma jet are studied.Firstly,results show that gas doping causes an increase in voltage and a decrease in current compared with the pure He discharge under the same discharge power,which might be attributed to the different chemical characteristics of O_2 and N_2 and verified by the changes in the gaseous reactive species shown in the optical emission spectroscopy(OES) and Fourier transform infrared(FTIR)spectroscopy.Secondly,the concentrations of aqueous reactive oxygen species(ROS) and reactive nitrogen species(RNS) are tightly related to the addition of O_2 and N_2 into the working gas.The concentrations of aqueous NO_2~- and NO_3~- significantly increase while the concentrations of aqueous ROS decrease with the admixture of N_2.The addition of O_2 has little effect on the concentrations of NO_2~- and NO_3~- and pH values; however,the addition of O_2 increases the concentration of O_2~- and deceases the concentrations of H_2O_2 and OH.Finally,the results of bactericidal experiments demonstrate that the inactivation efficiency of the four types of plasma jets is He?+?O_2??He+AirHeHe+N_2,which is in accordance with the changing trend of the concentration of aqueous O_2~-.Simultaneously to the better understanding of the formation and removal mechanisms of reactive species in the plasma–liquid interaction,these results also prove the effectiveness of regulating the concentrations of aqueous reactive species and the bacteria inactivation effects by gas doping.     

ESR法研究Pt催化N2H4分解机制

采用电子自旋共振谱（ESR）法,研究了酸性条件下•NH₂的转化,HClO₄体系下反应时间对溶液中自由基产生的影响、pH值对N₂H₄断键的影响以及HNO₃中N是否对溶液中的•NH₂有贡献,确定了Pt催化N₂H₄分解的反应机理。结果表明：在酸性条件下•NH₂被DMPO捕捉时反应式为•NH⁺₃+HO-H+DMPO=NH⁺₄+DMPO(•OH),硝酸在Pt催化N₂H₄体系中不会发生断键产生•NH₂,所产生的•NH₂是由N₂H₄断键形成的;在HClO₄体系中,随着Pt催化N₂H₄反应时间的延长,N₂H₄中N-N断键的趋势逐渐减小,N-H断键的趋势逐渐增大;随pH值的增大,N₂H₄中N-N断键的速率先快速减小,pH>3后缓慢增大;Pt催化N₂H₄分解反应中N-N断键和N-H断键两种方式共存,但N-N断键占优;反应体系中N₂H₄与H^＋浓度之比决定了N-N断键生成•NH₂的速率,而•NH₂与H^＋的浓度又决定了•NH₂转化成产物的速率,这两方面共同决定了N₂H₄分解的速率。     

N2 Mole Fraction Dependence of Plasma Bullet Propagation in Premixed He/N2 Plasma Needle Discharge at Atmospheric Pressure

In this work, a computational modeling study on the mechanism of the acceleration behavior of a plasma bullet in needle-plane configuration is presented. Above all, in our model,two sub-models of time-dependent plasma dynamics and laminar flow are connected using a oneway coupled method, and both the working gas and the surrounding gas around the plasma jet are assumed to be the same, which are premixed He/N_2 gas. The mole fractions of the N_2(NMF)ingredient are set to be 0.01%, 0.1% and 1% in three cases, respectively. It is found that in each case, the plasma bullet accelerates with time to a peak velocity after it exits the nozzle and then decreases until getting to the treated surface, and that the velocity of the plasma bullet increases at each time moment with the peak value changing from 0.72×10~6m/s to 0.80×10~6m/s but then drops more sharply when the NMF varies from 0.01% to 1%. Besides, the electron impact ionizations of helium neutrals and nitrogen molecules are found to have key influences on the propagation of a plasma bullet instead of the penning ionization.     

不同离子浓度对~(239)Pu在高庙子膨润土上的吸附影响

采用静态吸附法研究了239 Pu在CO2-3、HCO-3、SO2-4、Mg2+、Ca2+、Fe3+等不同离子浓度下在膨润土上的吸附。实验结果表明:随着CO2-3、HCO-3、Mg2+、Ca2+、Fe3+浓度的增大,239Pu在膨润土上的吸附分配系数Kd值逐渐减小,而随着SO2-4浓度的增加,Kd值先增加后减小,其中CO2-3、Fe3+浓度对Kd值影响较大。     

Low energy nitrogen ion doping into GaAs using combined ion-beam and molecular-beam epitaxy method

Low energy nitrogen (N) ions were irradiated during the epitaxial growth of GaAs using combined ion beam and molecular beam epitaxy (CIBMBE) method as a function of N⁺ ion acceleration energy (E_a) and N⁺ ion beam current density (I_N). E_a was varied from 70 to 170 eV I_N from 900 pA/cm² to 75 nA/cm². GaAs growth rate was fixed to 1 μm/h. In 2 K photoluminescence (PL) spectra of the samples with I_N = 3 nA/cm² and E_a = 70–100 eV, two sharp emissions at 1.508 eV (X₁) and 1.495 eV (X₂), which have been attributed to the emissions of excitons bound to isolated N atoms, and another one at 1.443 eV (X₅) were observed. These results show that nitrogen (N) atom in GaAs becomes optically active as an isoelectronic impurity at least in as-grown condition. For N⁺ ion-irradiated samples with rather high I_N, e.g., with I_N = 75 nA/cm² and E_a = 100 eV, a broad emission together with multiple sharp ones were observed after furnace annealing at 750°C which were ascribed to emissions of excitons bound to nitrogen-nitrogen (N---N) pairs.     

电喷雾串联质谱模拟天然单质铀的形成

采用三重四级杆质谱模拟并分析微观含铀分子化学键断裂形成新的物质的过程以探讨单质铀的产生机理。结果表明,含铀分子在质谱中离子化后经碰撞诱导解离可生成U⁺。研究还发现,硝酸铀酰溶液通过电喷雾可形成UO⁺₂(m/z 270)、UO₂OH⁺(m/z 287)、UO₂H₂OOH⁺(m/z 305)、UO₂NO⁺₃(m/z 332)、UO₂(H₂O)₃NO⁺₃(m/z 386)及双聚铀酰离子［(UO₂NO₃H₂O)₂NO₃］⁺(m/z 762),在具有一定动能N₂的碰撞下它们均可产生游离的U⁺。通过模拟实验推测,天然单质铀形成的微观机理为：在漫长地质年代中放射性核素持续衰变产生的能量粒子撞击含铀分子使其化学键断裂生成游离铀离子,在封闭或强还原性等特殊地质条件下形成单质铀并被保存下来。     

Time-Resolved Optical Emission Spectroscopy Diagnosis of CO2 Laser-Produced SnO2 Plasma

The spectral emission and plasma parameters of SnO_2 plasmas have been investigated.A planar ceramic SnO_2 target was irradiated by a CO2 laser with a full width at half maximum of 80 ns.The temporal behavior of the specific emission lines from the SnO_2 plasma was characterized.The intensities of Sn I and Sn II lines first increased,and then decreased with the delay time.The results also showed a faster decay of Sn I atoms than that of Sn II ionic species.The temporal evolutions of the SnO_2 plasma parameters(electron temperature and density) were deduced.The measured temperature and density of SnO_2 plasma are 4.38 eV to0.5 eV and 11.38×10~(17) cm~(-3) to 1.1×10~(17) cm~(-3),for delay times between 0.1 μs and 2.2 μs.We also investigated the effect of the laser pulse energy on SnO_2 plasma.     

Estimation of plasma density perturbation from dusty plasma injection by laser irradiation on tungsten target in DiPS

To investigate the interaction of dusty plasma with magnetized plasmas at divertor plasma simulator, radial profiles of plasma density(ne) and electron temperature were measured in terms of plasma discharge currents and magnetic flux intensity by using a fast scanning probes system with triple tips. Dusty plasma with dusts(a generation rate of 3 μg s~(-1) and a size of 1–10 μm)was produced via interactions between a high-power laser beam and a full tungsten target. As ne increases, the scale of the effects of dusty plasma injection on magnetized plasmas was decreased. Also, the duration of transient fluctuation was reduced. For numerical estimation of plasma density perturbation due to dusty plasma injection, the result was ~10% at a core region of the magnetized plasma with n_e of(2–5)×10~(11) cm~(-3) at steady state condition.     

Development of a helicon-wave excited plasma facility with high magnetic field for plasma-wall interactions studies

The high magnetic field helicon experiment system is a helicon wave plasma(HWP)source device in a high axial magnetic field(B_0)developed for plasma–wall interactions studies for fusion reactors.This HWP was realized at low pressure(5?×?10~(-3)?-?10 Pa)and a RF(radio frequency,13.56 MHz)power(maximum power of 2 k W)using an internal right helical antenna(5 cm in diameter by 18 cm long)with a maximum B_0of 6300 G.Ar HWP with electron density~10~(18)–10~(20)m~(-3)and electron temperature~4–7 e V was produced at high B_0 of 5100 G,with an RF power of 1500 W.Maximum Ar~+ion flux of 7.8?×?10~(23)m~(-2)s~(-1)with a bright blue core plasma was obtained at a high B_0 of 2700 G and an RF power of 1500 W without bias.Plasma energy and mass spectrometer studies indicate that Ar~+ion-beams of 40.1 eV are formed,which are supersonic(~3.1c_s).The effect of Ar HWP discharge cleaning on the wall conditioning are investigated by using the mass spectrometry.And the consequent plasma parameters will result in favorable wall conditioning with a removal rate of 1.1?×?10~(24)N_2/m~2 h.     

Temperature and dose dependences of nitrogen implantation into aluminium

It has been established that nitrogen implantation into metals can alter their surface properties such as friction, wear, corrosion, etc. Recent studies have shown that nitrogen implantation into aluminium leads to the formation of aluminium nitride which has interesting tribological, electronic and optical properties. For a given implantation energy, the characteristics of the nitrogen profile, e.g. thickness, shape and concentration, depend strongly on the experimental conditions during the implantation. In order to study the influence of the implantation parameters, aluminium samples have been bombarded with ¹⁵N⁺₂ of 100 keV to different doses ((1–20) × 10¹⁷ N⁺/cm²), at several temperatures (25–300° C). Distributions of the implanted species were investigated by nuclear reaction analysis (NRA) and by Rutherford backscattering spectroscopy (RBS). The chemical bonds of aluminium in the matrix were studied by using low-energy electron-induced X-ray spectroscopy (LEEIXS). It is shown that aluminium nitride is formed and that the nitrogen distribution presents a surface peak when the implantation temperature is higher than 200° C.     

Ion implantation doping and electrical conductivity enhancement of C60 films

Pristine C₆₀ films sublimed onto sheet mica were implanted with 20 keV K⁺ ions and I⁺ ions at doses of 1.0 × 10¹⁶/cm², 3.0 × 10¹⁶/cm² and 5.0 × 10¹⁶/cm², and with 20 keV Ar⁺ ions at a dose of 5.0 × 10¹⁶/cm². The distributions of dopants were studied using Rutherford backscattering spectrometry (RBS). The temperature dependence of sheet resistivity of the films was investigated applying a four-probe system. It was proposed that the conductivity enhancement of K⁺ implanted C₆₀ films was due to the implanted ions in the films, while for I⁺ implanted C₆₀ films, both implanted I⁺ ions and irradiation effects of the ions contributed to the enhancement of conductivity.     

Am在两种不同地下水中的种态分布及溶解度分析

利用自主编写的地球化学计算软件CHEMSPEC分析了Am在北山地下水和我国西南某地下水中的种态分布,并计算了Am在这两种地下水中的溶解度,考察了pH、Eh、不同离子以及硅的存在等对种态分布的影响。结果表明,Am在这两种地下水中均以正三价存在,随pH值的不同Am的种态会发生较大的变化,在偏酸性条件下,主要以AmSO+4、Am(SO4)-2及Am3+的形式存在,在中性至弱碱性条件下,以AmCO+3的形式存在,强碱性条件下,则基本转化为Am(OH)3;当北山地下水中有Si存在时,在pH=6.5~9.7范围内,Am的主要种态为AmSiO(OH)2+3;不同离子的浓度变化对Am的种态分布会产生一定影响,其影响顺序为HCO-3F-SO2-4Cl-。pH和HCO-3对Am溶解度的影响较大,随着地下水pH的升高,Am的溶解度逐渐减小。Am在两种地下水中的溶解度分别为2.01×10-7 mol/L(北山地下水pH=7.56、Eh=164mV)、1.60×10-7 mol/L(西南地下水pH=7.50、Eh=0mV)。     

Measurement ofHe2* density with an auxiliary measuring electrode in atmospheric pressure plasma jet

In this study, the density of metastable He₂* in an atmospheric-pressure plasma jet operating in helium with 0.001% nitrogen has been measured using an auxiliary measuring electrode technique. In the glow discharge mode, waveforms from two grounding electrodes, including one main discharge electrode and one auxiliary electrode, are captured. The isolated current peak formed by Penning ionization in waveforms from the auxiliary measuring electrode is identified to calculate the density of metastable He₂*. In our discharge environment, the helium metastable densities along the jet axis direction are between 2.26× 10¹³ and 1.74× 10¹³ cm^-3, which is in good agreement with the results measured by other techniques. This measurement technique can be conveniently applied to the diagnosis of metastableHe₂* in an atmospheric-pressure plasma jet array.     

Evaluation of trans-ferulic acid degradation by dielectric barrier discharge plasma combined with ozone in wastewater with different water quality conditions

In this study, dielectric barrier discharge plasma and ozone(O_3) were combined to synergistically degrade trans-ferulic acid(FA), and the effect of water quality on FA degradation was studied. The results showed that 96.9% of FA was degraded after 40 min treatment by the plasma/O_3 process. FA degradation efficiency increased with the p H values. The presence of suspended solid and humic acid inhibited FA degradation. FA degradation efficiency increased as the water temperature increased to 30 °C. However, the further increase in water temperature was adverse for FA degradation. Effects of common inorganic ions on FA degradation were also investigated. The addition of Cl~- inhibited the FA degradation, whileCO_3~(2-) had both negative and positive influences on FA degradation.NO_3~- andSO_4~(2-) did not have significant effect on FA degradation. Fe~(3+)and Cu~(2+)benefited FA degradation through the Fenton-like and catalytic ozonation reactions.     

Numerical investigation on electron effects in the mass transfer of the plasma species in aqueous solution

The objective of this work is to contribute an understanding of the effects of electrons in the plasmas on the mass transfer of plasma species in aqueous solution by means of the numerical simulation based on a one-dimensional diffusion-reaction model. The plasma species are divided into two groups, i.e. electrons and the other species, and the mass transfer in the three scenarios has been simulated, including the systematic calculations of the depth distributions of five major reactive species, OH, O₃, HO₂ , O₂^-, and H₂O₂ . In the three scenarios, the particles considered to enter into aqueous solution are all the plasma species (the scenario I, where the mass transfer of plasma species is a result due to the synergy of the electrons and the other plasma species), the other species (the scenario II), and only electrons in plasma species (the scenario III), respectively. The detailed analyses on the difference between the depth distributions of each reactive species in these three scenarios show the following conclusions. The electrons play an important role in the mass transfer of plasma species in aqueous solution and the synergy of the electrons and the other plasma species (the electron-species synergy) presents its different effects on the mass transfer. The vast majority of H₂O₂ are generated from a series of the electron- related reactions in aqueous solution, which is hardly affected by the electron-species synergy. Compared to the results when only the electrons enter into the liquid region, the electron-species synergy evidently weakens the generation of O₂^-, O₃ , and OH, but promotes to produce HO₂ .     

硝酸体系中铂催化肼还原U(Ⅵ)的反应动力学

开展了硝酸体系中以肼为还原剂、铂黑为催化剂催化还原U(Ⅵ)的动力学研究。通过考察U(Ⅵ)浓度、肼浓度、酸度以及催化剂用量等条件对反应过程的影响，确定了反应的初始动力学速率方程为-dc(UO²⁺₂)dt=kc^0.44(UO²⁺₂)c^0.19(N₂H⁺₅)c^-0.23(H⁺)，在60 ℃、固液比r_S/L=2.0 g/L时，速率常数k=2.6×10^-3 (mol/L)^0.6/min。研究了温度对反应速率的影响，结果表明，在20~75 ℃范围内，随着温度升高，反应速率加快，反应过程由动力学控制转变为扩散控制过程。对比了硝酸体系与高氯酸体系的反应动力学实验数据，发现相同条件下硝酸体系的反应速率明显低于高氯酸体系，并分析了其中的原因。     

硝酸体系中铂催化肼还原U(Ⅵ)的反应动力学

开展了硝酸体系中以肼为还原剂、铂黑为催化剂催化还原U(Ⅵ)的动力学研究。通过考察U(Ⅵ)浓度、肼浓度、酸度以及催化剂用量等条件对反应过程的影响,确定了反应的初始动力学速率方程为-dc(UO²⁺₂)dt=kc^0.44(UO²⁺₂)c^0.19(N₂H⁺₅)c^-0.23(H⁺),在60 ℃、固液比r_S/L=2.0 g/L时,速率常数k=2.6×10^-3 (mol/L)^0.6/min。研究了温度对反应速率的影响,结果表明,在20~75 ℃范围内,随着温度升高,反应速率加快,反应过程由动力学控制转变为扩散控制过程。对比了硝酸体系与高氯酸体系的反应动力学实验数据,发现相同条件下硝酸体系的反应速率明显低于高氯酸体系,并分析了其中的原因。     

Volume added surface barrier discharge plasma excited by bipolar nanosecond pulse power in atmospheric air: optical emission spectra influenced by gap distance

In this paper, volume barrier discharge with different gap distances is added on the discharge border of high-voltage electrode of annular surface barrier discharge for generating volume added surface barrier discharge (V-SBD) excited by bipolar nanosecond high-voltage pulse power in atmospheric air. The excited V-SBDs consist of surface barrier discharge (d=0 mm) and volume added surface barrier discharges (d=2 mm and 3 mm). The optical emission spectra are recorded for calculating emission intensities of N₂ (C ³Ⅱ_u →B³Π_g ) and N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ ), and simulating rotational and vibrational temperatures. The influences of gap distance of V-SBD on emission intensity and plasma temperature are also investigated and analyzed. The results show that d=0 mm structure can excite the largest emission intensity of N ₂ (C ³ Π_u →B ³Π_g ), while the existence of volume barrier discharge can delay the occurrence of the peak value of the emission intensity ratio of N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ )/N ₂(C³Π_u →B³Π_g ) during the rising period of the applied voltage pulse and weaken it during the end period. The increasing factor of emission intensity is effected by the pulse repetition rate. The d=3 mm structure has the highest threshold voltage while it can maintain more emission intensity of N₂(C³ Π _u →B ³Π_g ) than that of d=2 mm structure. The structure of d=2 mm can maintain more increasing factor than that of the d=3 mm structure with varying pulse repetition rate. Besides, the rotational temperatures of three V-SBD structures are slightly affected when the gap distance and pulse repetition rate vary. The vibrational temperatures have decaying tendencies of all three structures with the increasing pulse repetition rate.     

钙-铀-碳酸络合物对红土吸附铀性能的影响

采用静态实验法研究了钙-铀-碳酸络合物对红土吸附铀性能的影响。结果表明:溶液的pH值、总碳酸和钙离子浓度增大会抑制红土对铀的吸附,当pH=7.0,红土投加量为1g/L,钙离子、总碳酸根和初始铀浓度分别为0.4mmol/L、3.8mmol/L和50mg/L时,红土对铀的最大吸附容量约为4.20mg/g。铀在红土上的吸附形态为UO2(CO3)2-2、UO2(CO3)4-3和UO2CO3(aq)。利用铀-碳酸络合物总量c(UCO3)T可预测红土吸附铀的容量qe,c(U-CO3)T与qe呈非线性关系,其方程为qe=18.2(c(UO2+2)·c(CO2-3)(K1+K2c(CO2-3)+K3c2(CO2-3)))0.36。该研究成果可为铀污染土壤的修复和治理提供技术和理论参考。